Recently, air plasma, produced by focusing an intense laser beam to ionize atoms or molecules, has been demonstrated to be a promising source of broadband terahertz waves. However, simultaneous broadband and coherent detection of such broadband terahertz waves is still challenging. Electro-optical sampling and photoconductive antennas are the typical approaches for terahertz wave detection. The bandwidth of these detection methods is limited by the phonon resonance or carrier’s lifetime. Unlike solid-state detectors, gaseous sensors have several unique features, such as no phonon resonance, less dispersion, no Fabry-Perot effect, and a continuous renewable nature. The aim of this article is to review the development of a broadband terahertz time-domain spectrometer, which has both a gaseous emitter and sensor mainly based on author’s recent investigation. This spectrometer features high efficiency, perceptive sensitivity, broad bandwidth, adequate signal-to-noise ratio, sufficient dynamic range, and controllable polarization.
The detection of terahertz waves with ambient air has been realized through a third order nonlinear optical process: detecting the second harmonic photon that is produced by mixing one terahertz photon with two fundamental photons. In this review, a systematic investigation of the mechanism of broadband terahertz wave detection was presented first. The dependence of the detection efficiency on probe pulse energy, bias field strength, gas pressure and third order nonlinear susceptibility of gases were experimentally demonstrated with selected gases. Detailed discussions of phase matching and Gouy phase shift were presented by considering the focused condition of Gaussian beams. Furthermore, the bandwidth dependence on probe pulse duration was also demonstrated. Over 240 times enhancement of dynamic range had been accomplished with n-hexane vapor compared to conventional air sensor. Moreover, with sub-20 fs laser pulses delivered from a hollow fiber pulse compressor, an ultra-broad spectrum covering from 0.3 to 70 THz was also showed.
In addition, a balanced detection scheme using a polarization dependent geometry was developed by author to improve signal-to-noise ratio and dynamic range of conventional terahertz air-biased-coherent-detection (ABCD) systems. Utilizing the tensor property of third order nonlinear susceptibility, second harmonic pulses with two orthogonal polarizations was detected by two separated photomultiplier tubes (PMTs). The differential signal from these two PMTs offers a realistic method to reduce correlated laser fluctuation, which circumvents signal-to-noise ratio and dynamic range of conventional terahertz ABCD systems. A factor of two improvement of signal-to-noise ratio was experimentally demonstrated.
This paper also introduces a unique approach to directly produce a broadband elliptically polarized terahertz wave from laser-induced plasma with a pair of double helix electrodes. The theoretical and experimental results demonstrated that velocity mismatch between excitation laser pulses and generated terahertz waves plays a key role in the properties of the elliptically polarized terahertz waves and confirmed that the far-field terahertz emission pattern is associated with a coherent process. The results give insight into the important influence of propagation effects on terahertz wave polarization control and complete the mechanism of terahertz wave generation from laser-induced plasma.
This review provides a critical understanding of broadband terahertz time-domain spectroscopy (THz-TDS) and introduces further guidance for scientific applications of terahertz wave gas photonics.
Terahertz (THz) wave science and technology have been found countless applications in biomedical imaging, security screening, and non-destructive testing as they approach maturity. However, due to the challenge of high ambient moisture absorption, the development of remote open-air broadband THz spectroscopy technology is lagging behind the compelling need that exists in homeland security, astronomy and environmental monitoring. Furthermore, the underlying physical mechanisms behind the interaction between the THz wave and laser-induced plasma which responds strongly to electromagnetic waves have not been fully understood.
This review aims to explain the light-plasma interaction at THz frequencies within a semiclassical framework along with experimental study of the femtosecond-laser-induced nitrogen plasma fluorescence under the illumination of single-cycle THz pulses. The results indicate that THz-radiation-enhanced-emission-of-fluorescence (THz-REEF) is dominated by electron kinetics in the THz field and the electron-impact excitation of gas molecules/ions. The information of the time-dependent THz field can be recovered from the measured time-resolved THz-REEF from single-color laser induced plasma with the help of the bias as local oscillator. The calculations and experimental verification lead to complete understanding of the science behind these effects and push forward to extend their capabilities in related applications such as remote THz sensing, plasma diagnostics and ultrafast photoluminescence modulation.
Systematic studies in selected gases including neon, argon, krypton, xenon, methane (CH4), ethane (C2H6), propane (C3H8), and n-butane (C4H10) gases were performed to obtain an improved understanding of the THz-REEF. The dependences of the enhanced fluorescence on the THz field, laser excitation intensity, gas pressure, and intrinsic atomic properties were experimentally characterized. Both narrow line emission and broad continuum emission of the gas plasma were enhanced by the THz field. Their fluorescence enhancement ratios and time-resolved enhanced fluorescence were largely dependent on the scattering cross section and ionization potential of atoms.
For the first time, we demonstrated a novel ‘all-optical’ technique of broadband THz wave remote sensing by coherently manipulating the fluorescence emission from asymmetrically ionized gas plasma that interacted with THz waves. By studying the ultrafast electron dynamics under the single cycle THz radiation, we found that the fluorescence emission from laser-induced air plasma was highly dependent on the THz electric field and the symmetry of the electron drift velocity distribution created by two-color laser fields. The time-resolved THz-REEF can be tailored by switching the relative two-color phase and laser polarizations. Owing to the high atmospheric transparency and omni-directional emission pattern of fluorescence, this technique can be used to measure THz pulses at standoff distances with minimal water vapor absorption and unlimited directionality for optical signal collection. The coherent THz wave detection at a distance of 10 m had been demonstrated. The combination of this method and previously demonstrated remote THz generation would eventually make remote THz spectroscopy available.
We also introduced a unique plasma diagnostic method utilizing the THz-wave-enhanced fluorescence emission from the excited atoms or molecules. The electron relaxation time and plasma density were deduced through applying the electron impact excitation/ionization and electron-ion recombination processes to the measured time-delay-dependent enhanced fluorescence. The electron collision dynamics of nitrogen plasma excited at different gas pressures and laser pulse energies were systematically investigated. This plasma diagnostic method offers picosecond temporal resolution and is capable of omni-directional optical signal collection.
The ultrafast quenching dynamics of laser-pulse-induced photoluminescence in semiconductors under the radiation of single-cycle THz pulses was studied. It was found that the quenching in both cadmium telluride (CdTe) and gallium arsenide (GaAs) was linearly proportional to the intensity of incident THz waves and reaches up to 17% and 4% respectively at the peak intensity of 13 MW/cm2. The THz-wave-induced heating of the carriers and lattice and the subsequent decreased efficiency of photocarrier generation and recombination were most likely to be responsible for the quenching. This is potentially useful for the applications of a non-invasive ultrafast light modulator for photoluminescence devices with picoseconds switching time in the fields of the light-emitting devices and optical communication.
This paper studies laser air-photonics used for remote sensing of short pulses of electromagnetic radiation at terahertz frequency. Through the laser ionization process, the air is capable of generating terahertz field strengths greater than 1 MV/cm, useful bandwidths over 100 terahertz, and highly directional emission patterns. Following ionization and plasma formation, the emitted plasma acoustic or fluorescence can be modulated by an external terahertz field to serve as omnidirectional, broadband, electromagnetic sensor. These results help to close the “terahertz gap” once existing between electronic and optical frequencies, and the acoustic and fluorescence detection methodologies developed provide promising new avenues for extending the useful range of terahertz wave technology. Our experimental results indicate that by hearing the sound or seeing the fluorescence, coherent detection of broadband terahertz wave at remote distance is feasible.
Semiconductor nonlinearity in the range of terahertz (THz) frequency has been attracting considerable attention due to the recent development of high-power semiconductor-based nanodevices. However, the underlying physics concerning carrier dynamics in the presence of high-field THz transients is still obscure. This paper introduces an ultrafast, time-resolved THz pump/THz probe approach to study semiconductor properties in a nonlinear regime. The carrier dynamics regarding two mechanisms, intervalley scattering and impact ionization, was observed for doped InAs on a sub-picosecond time scale. In addition, polaron modulation driven by intense THz pulses was experimentally and theoretically investigated. The observed polaron dynamics verifies the interaction between energetic electrons and a phonon field. In contrast to previous work which reported optical phonon responses, acoustic phonon modulations were addressed in this study. A further understanding of the intense field interacting with solid materials will accelerate the development of semiconductor devices.
This paper can be divided into 4 sections. Section 1 starts with the design and performance of a table-top THz spectrometer, which has the advantages of ultra-broad bandwidth (one order higher bandwidth compared to a conventional ZnTe sensor) and high electric field strength (>100 kV/cm). Unlike the conventional THz time-domain spectroscopy, the spectrometer integrated a novel THz air-biased-coherent-detection (THz-ABCD) technique and utilized gases as THz emitters and sensors. In comparison with commonly used electro-optic (EO) crystals or photoconductive (PC) dipole antennas, the gases have the benefits of no phonon absorption as existing in EO crystals and no carrier life time limitation as observed in PC dipole antennas. In Section 2, the newly development THz-ABCD spectrometer with a strong THz field strength capability provides a platform for various research topics especially on the nonlinear carrier dynamics of semiconductors. Two mechanisms, electron intervalley scattering and impact ionization of InAs crystals, were observed under the excitation of intense THz field on a sub-picosecond time scale. These two competing mechanisms were demonstrated by changing the impurity doping type of the semiconductors and varying the strength of the THz field.
Another investigation of nonlinear carrier dynamics in Section 3 was the observation of coherent polaron oscillation in n-doped semiconductors excited by intense THz pulses. Through modulations of surface reflection with a THz pump/THz probe technique, this work experimentally verifies the interaction between energetic electrons and a phonon field, which has been theoretically predicted by previous publications, and shows that this interaction applies for the acoustic phonon modes. Usually, two transverse acoustic (2TA) phonon responses are inactive in infrared measurement, while they are detectable in second-order Raman spectroscopy. The study of polaron dynamics, with nonlinear THz spectroscopy (in the far-infrared range), provides a unique method to diagnose the overtones of 2TA phonon responses of semiconductors, and therefore incorporates the abilities of both infrared and Raman spectroscopy. Finally, some conclusions were presented in Section 4. In a word, this work presents a new milestone in wave-matter interaction and seeks to benefit the industrial applications in high power, small scale devices.
Undesired reflection caused by impedance mismatch can lead to significant power loss and other unwanted effects. In the terahertz regime, anti-reflection method has evolved from simple quarter-wave anti-reflection coating to sophisticated metamaterial device and photonic structures. In this paper, we examined and compared the theories and techniques of several anti-reflection implementations for terahertz waves, with emphasis on gradient index photonic structures. A comprehensive study is presented on the design, fabrication and evaluation of this new approach.